Engineering the Compositional Architecture of Core‐Shell Upconverting Lanthanide‐Doped Nanoparticles for Optimal Luminescent Donor in Resonance Energy Transfer: The Effects of Energy Migration and Storage

Förster Resonance Energy Transfer (FRET) between single molecule donor (D) and acceptor (A) is well understood from a fundamental perspective and is widely applied in biology, biotechnology, medical diagnostics, and bio‐imaging. Lanthanide doped upconverting nanoparticles (UCNPs) have demonstrated t...

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Bibliographic Details
Published in:Small (Weinheim an der Bergstrasse, Germany) Germany), 2022-05, Vol.18 (18), p.e2200464-n/a
Main Authors: Pilch‐Wrobel, Aleksandra, Kotulska, Agata Maria, Lahtinen, Satu, Soukka, Tero, Bednarkiewicz, Artur
Format: Article
Language:English
Subjects:
biosensors
Bleaching
Decay
Energy storage
Energy transfer
Erbium
Excitation spectra
Fluorescence Resonance Energy Transfer - methods
Förster resonance energy transfer
Ions
lanthanide doped nanoparticles
Lanthanoid Series Elements
Luminescence
Nanoparticles
Nanotechnology
photon upconversion
Resonance
Ytterbium
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Summary:Förster Resonance Energy Transfer (FRET) between single molecule donor (D) and acceptor (A) is well understood from a fundamental perspective and is widely applied in biology, biotechnology, medical diagnostics, and bio‐imaging. Lanthanide doped upconverting nanoparticles (UCNPs) have demonstrated their suitability as alternative donor species. Nevertheless, while they solve most disadvantageous features of organic donor molecules, such as photo‐bleaching, spectral cross‐excitation, and emission bleed‐through, the fundamental understanding and practical realizations of bioassays with UCNP donors remain challenging. Among others, the interaction between many donor ions (in donor UCNP) and many acceptors anchored on the NP surface and the upconversion itself within UCNPs, complicate the decay‐based analysis of D‐A interaction. In this work, the assessment of designed virtual core‐shell NP (VNP) models leads to the new designs of UCNPs, such as …@Er, Yb@Er, Yb@YbEr, which are experimentally evaluated as donor NPs and compared to the simulations. Moreover, the luminescence rise and decay kinetics in UCNP donors upon RET is discussed in newly proposed disparity measurements. The presented studies help to understand the role of energy‐transfer and energy migration between lanthanide ion dopants and how the architecture of core‐shell UCNPs affects their performance as FRET donors to organic acceptor dyes. The compositional architecture of lanthanide‐doped upconverting core‐shell nanoparticles (UCNPs) strongly affects their suitability for Resonant Energy Transfer (RET) based sensing. The upconversion (UC) in lanthanides advantageously diminishes background signal, but concurrently complicates luminescence kinetics analysis. Newly suggested RET quantification methods exploit long luminescence risetimes of the donor and fluorescent acceptor molecules to understand the mechanisms behind and propose optimized donor NPs.
ISSN:1613-6810
1613-6829
DOI:10.1002/smll.202200464